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NMR spin-lattice relaxation time (T1) measurements were performed for 14N of acetonitrile in acetonitrile (CH3CN)—H2O mixtures and for 2H of heavy water in CH3CN—D2O mixtures at 30°C up to 294.2 MPa together with those for 2H in CH3CN—D2O mixtures at 10 and 20°C under atmospheric pressure over the whole composition range of the mixtures. IR absorption spectra for CH3CN—H2O and CH3CN—10 mol% HDO/D...